Mesoporous Metal–Nitrogen-Doped Carbon Electrocatalysts for Highly Efficient Oxygen Reduction Reaction

• Published in: Journal of the American Chemical Society Vol. 135; no. 43; pp. 16002 - 16005
• Main Authors: Liang, Hai-Wei, Wei, Wei, Wu, Zhong-Shuai, Feng, Xinliang, Müllen, Klaus
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 30.10.2013
• Subjects: active sites; carbon; catalysts; chemical reduction; electrochemistry; electron transfer; montmorillonite; nanoparticles; oxygen; porous media; silica; surface area; vitamin B12
• ISSN: 0002-7863; 1520-5126; 1520-5126
• DOI: 10.1021/ja407552k

A family of mesoporous nonprecious metal (NPM) catalysts for oxygen reduction reaction (ORR) in acidic media, including cobalt–nitrogen-doped carbon (C–N–Co) and iron–nitrogen-doped carbon (C–N–Fe), was prepared from vitamin B12 (VB12) and the polyaniline-Fe (PANI-Fe) complex, respectively. Silica nanoparticles, ordered mesoporous silica SBA-15, and montmorillonite were used as templates for achieving mesoporous structures. The most active mesoporous catalyst was fabricated from VB12 and silica nanoparticles and exhibited a remarkable ORR activity in acidic medium (half-wave potential of 0.79 V, only ∼58 mV deviation from Pt/C), high selectivity (electron-transfer number >3.95), and excellent electrochemical stability (only 9 mV negative shift of half-wave potential after 10 000 potential cycles). The unprecedented performance of these NPM catalysts in ORR was attributed to their well-defined porous structures with a narrow mesopore size distribution, high Brunauer–Emmett–Teller surface area (up to 572 m2/g), and homogeneous distribution of abundant metal–N x active sites.